A dye sensitized photosynthesis cell for stable water oxidation mediated by photo-generated bromine
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The water oxidation process at the sensitization–oxidation photo-anode by photo-generated bromine.Keywords:
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Metal oxides with moderate band gaps are desired for efficient production of hydrogen from sunlight and water via photoelectrochemical (PEC) water splitting. Here, we report an α-SnWO4 photoanode synthesized by hydrothermal conversion of WO3 films that achieves photon to current conversion at wavelengths up to 700 nm (1.78 eV). This photoanode is promising for overall PEC water-splitting because the flat-band potential and voltage of photocurrent onset are more negative than the potential of hydrogen evolution. Furthermore, the photoanode utilizes a large portion of the solar spectrum. However, the photocurrent density reaches only a small fraction of that which is theoretically possible. Density functional theory based thermodynamic and electronic structure calculations were performed to elucidate the nature and impact of defects in α-SnWO4 prepared by this synthetic route, from which hole localization at Sn-at-W antisite defects was determined to be a likely cause for the poor photocurrent. Measurements further showed that the photocurrent decreases over time due to surface oxidation, which was suppressed by improving the kinetics of hole transfer at the semiconductor/electrolyte interface. Alternative synthetic methods and the addition of protective coatings and/or oxygen evolution catalysts are suggested to improve the PEC performance and stability of this promising α-SnWO4 material.
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Highly photoactive and durable photoanode materials are the key to photoelectrochemical water splitting. In this paper, hierarchically branched Fe2O3@TiO2 nanorod arrays (denoted as Fe2O3@TiO2 BNRs) composed of a long Fe2O3 trunk and numerous short TiO2 nanorod branches were fabricated and used as photoanodes for water splitting. Significant improvement of photoelectrochemical water splitting performance was observed based on Fe2O3@TiO2 BNRs. The photocurrent density of Fe2O3@TiO2 BNRs reaches up to 1.3 mA cm(-2) at 1.23 V versus RHE, which is 10 times higher than that of pristine Fe2O3 nanorod arrays under the same conditions. Furthermore, an obvious cathodic shift in the onset potential of photocurrent was observed in the Fe2O3@TiO2 BNRs. More significantly, the Fe2O3@TiO2 BNRs are quite stable even after 3600 s continuous illumination, and the photocurrent density shows almost no decay. Finally, a tentative mechanism was proposed to explain the superior performance of Fe2O3@TiO2 BNRs for PEC water splitting and discussed in detail on the basis of our experimental results.
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Photocatalytic water splitting
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n-Cu2O photoelectrodes were fabricated by boiling a copper plate for 60 min in a CuSO4 (10−3M) solution. A photocurrent enhancement was found in the photoelectrochemical cell after the potential sweeping of the samples in the presence of water as the electrolyte. The reason for the photocurrent enhancement was found by depletion of the surface states on n-Cu2O at electrolyte interface by potential sweeping.
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High performance and toxicity assessment of Ta3N5 nanotubes for photoelectrochemical water splitting
In this work, Co-based cocatalysts are electrodeposited on mesoporous Ta3N5 nanotubes. The electrodeposition time is varied and the optimized photoelectrode reaches a photocurrent density of 6.3 mA/cm2 at 1.23 V vs. SHE, under simulated solar illumination of 1 Sun, in 1 M NaOH. The best performing electrode, apart from the high photocurrent density, shows improved stability under intense photoelectrochemical water splitting conditions. The dual function of the cocatalyst to improve not only the photoelectrochemical performance, but also the stability, is highlighted. Moreover, we adopted a simple protocol to assess the toxicity of Co and Ta contained nanostructured materials (representing used photoelectrodes) employing the human cell line HeLa S3 as target cells.
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Here we show that in dye-sensitized solar cells a lanthanum post treatment of mesoporous TiO2 electrodes increases either the photovoltage or the photocurrent, depending on the solution pH. With an electrode treatment at pH 7, the photovoltage increase is compensated by a decrease in the photocurrent, leading to slightly reduced conversion efficiency. With an acidic post treatment, the photocurrent increases by 20–25% while the photovoltage remains unchanged. As a result, an improvement of the light to electric power conversion efficiency from 5.6 to 7.0% is achieved. The same behavior is observed when lanthanum acetate is added to the commonly used TiCl4 post-treatment, where the observed efficiency increase is significantly higher compared with TiCl4-treated electrodes without lanthanum.
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Photoanodes made from BaTaO2N that can harvest visible light up to 660 nm wavelength were fabricated on Ti substrates for achieving efficient water splitting. Both pre-treatment of BaTaO2N particles with an H2 stream and post-necking treatment with TaCl5 effectively increased the photocurrent due to the decreased electrical resistance in the porous BaTaO2N photoanode. A combination of pre-loading of CoO(x) on the BaTaO2N particles and post-loading of RhO(x) significantly improved both the photocurrent and stability under visible light irradiation, along with an obvious negative shift (ca. 300 mV) of the onset potential for water oxidation, while sole loading resulted in a lower photocurrent or insufficient stability. The IPCE value was estimated to be ca. 10% at 1.2 V vs RHE under 600 nm, which is the highest among photoanode materials that can harvest light beyond 600 nm for water oxidation. Photoelectrochemical water splitting into H2 and O2 under visible light was demonstrated using RhO(x)/CoO(x)/BaTaO2N/Ti photoanodes under an externally applied bias larger than 0.7 V to a Pt counter electrode.
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In this Reply, Niederberger responds to the Comment written by Augustynski and Solarska regarding the article entitled “Commercially Available WO3 Nanopowders for Photoelectrochemical Water Splitting: Photocurrent versus Oxygen Evolution” (ChemPlusChem 2016, 81, 935–940).
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